Breaking the Linear Scaling Relationship of the Reverse Water–Gas–Shift Reaction via Construction of Dual-Atom Pt–Ni Pairs
Yajing Wang, Jianmin Chen, Liyu Chen, Yingwei Li
Abstract
Oxide-supported single-atom catalysts hold great potential for reverse water–gas–shift (RWGS) reactions. Nevertheless, it remains challenging to break the linear scaling relationships between the adsorption and desorption capability of catalysts. Herein, we report the design of ZrO 2 -anchored dual-atom Pt–Ni pairs for the RWGS reaction. The dual-atom material delivers a CO selectivity as high as 99.8% and a space-time yield of 157.2 μmol CO g cat –1 s –1 at atmospheric pressure. Theoretical calculations reveal that the dual-atom Pt–Ni pairs could direct the dual electronic transfer paths (d xz and d yz ) to the 2π* orbitals of CO 2 in the RWGS reaction, which achieve strong hybridization between them to enable efficient activation of CO 2 . Moreover, the delocalized charge in dual-atom Pt–Ni may lead to a facile desorption of the CO product.